CN106076312B - A kind of Nb (OH)5Nano wire/redox graphene composite photo-catalyst and the preparation method and application thereof - Google Patents
A kind of Nb (OH)5Nano wire/redox graphene composite photo-catalyst and the preparation method and application thereof Download PDFInfo
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 87
- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 86
- 239000002131 composite material Substances 0.000 title claims abstract description 73
- 239000011941 photocatalyst Substances 0.000 title claims abstract description 61
- 238000002360 preparation method Methods 0.000 title claims abstract description 34
- 239000002070 nanowire Substances 0.000 claims abstract description 77
- 230000009467 reduction Effects 0.000 claims abstract description 30
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 claims abstract description 27
- 238000006243 chemical reaction Methods 0.000 claims abstract description 21
- ZKATWMILCYLAPD-UHFFFAOYSA-N niobium pentoxide Inorganic materials O=[Nb](=O)O[Nb](=O)=O ZKATWMILCYLAPD-UHFFFAOYSA-N 0.000 claims abstract description 16
- 238000000034 method Methods 0.000 claims abstract description 14
- 239000003344 environmental pollutant Substances 0.000 claims abstract description 10
- -1 graphene compound Chemical class 0.000 claims abstract description 10
- 231100000719 pollutant Toxicity 0.000 claims abstract description 10
- 239000002351 wastewater Substances 0.000 claims abstract description 10
- 239000000725 suspension Substances 0.000 claims description 24
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 22
- 238000002156 mixing Methods 0.000 claims description 16
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 16
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 16
- 239000007787 solid Substances 0.000 claims description 16
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 15
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 10
- 238000001035 drying Methods 0.000 claims description 10
- 206010013786 Dry skin Diseases 0.000 claims description 8
- 239000008367 deionised water Substances 0.000 claims description 8
- 229910021641 deionized water Inorganic materials 0.000 claims description 8
- 239000000706 filtrate Substances 0.000 claims description 8
- 238000002604 ultrasonography Methods 0.000 claims description 8
- 239000000843 powder Substances 0.000 claims description 7
- 238000007789 sealing Methods 0.000 claims description 7
- 239000000084 colloidal system Substances 0.000 claims description 5
- 238000003756 stirring Methods 0.000 claims description 5
- 238000005286 illumination Methods 0.000 claims description 4
- 239000003795 chemical substances by application Substances 0.000 claims description 3
- JOPOVCBBYLSVDA-UHFFFAOYSA-N chromium(6+) Chemical compound [Cr+6] JOPOVCBBYLSVDA-UHFFFAOYSA-N 0.000 claims description 3
- 238000009826 distribution Methods 0.000 claims description 3
- 239000010955 niobium Substances 0.000 abstract description 79
- 239000011651 chromium Substances 0.000 abstract description 40
- 239000003054 catalyst Substances 0.000 abstract description 22
- 229910052804 chromium Inorganic materials 0.000 abstract description 12
- 230000005855 radiation Effects 0.000 abstract description 11
- 229910052758 niobium Inorganic materials 0.000 abstract description 9
- 239000002253 acid Substances 0.000 abstract description 8
- 230000015572 biosynthetic process Effects 0.000 abstract description 5
- 230000008569 process Effects 0.000 abstract description 5
- 238000003786 synthesis reaction Methods 0.000 abstract description 5
- 239000000463 material Substances 0.000 abstract description 4
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 abstract description 3
- 238000011065 in-situ storage Methods 0.000 abstract description 3
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 abstract description 3
- 230000002194 synthesizing effect Effects 0.000 abstract description 3
- 238000004519 manufacturing process Methods 0.000 abstract description 2
- GPRLSGONYQIRFK-UHFFFAOYSA-N hydron Chemical compound [H+] GPRLSGONYQIRFK-UHFFFAOYSA-N 0.000 abstract 1
- 229910021645 metal ion Inorganic materials 0.000 abstract 1
- 238000000746 purification Methods 0.000 abstract 1
- 231100000331 toxic Toxicity 0.000 abstract 1
- 230000002588 toxic effect Effects 0.000 abstract 1
- 239000000243 solution Substances 0.000 description 27
- 230000015556 catabolic process Effects 0.000 description 13
- 238000006731 degradation reaction Methods 0.000 description 13
- 230000001699 photocatalysis Effects 0.000 description 11
- 239000011521 glass Substances 0.000 description 10
- 230000000593 degrading effect Effects 0.000 description 9
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 7
- LINPIYWFGCPVIE-UHFFFAOYSA-N 2,4,6-trichlorophenol Chemical compound OC1=C(Cl)C=C(Cl)C=C1Cl LINPIYWFGCPVIE-UHFFFAOYSA-N 0.000 description 6
- 238000001816 cooling Methods 0.000 description 6
- 230000003287 optical effect Effects 0.000 description 6
- 150000007513 acids Chemical class 0.000 description 5
- 238000001354 calcination Methods 0.000 description 5
- 239000002086 nanomaterial Substances 0.000 description 5
- 238000007146 photocatalysis Methods 0.000 description 5
- 229910052724 xenon Inorganic materials 0.000 description 5
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 5
- 150000002989 phenols Chemical class 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 230000003197 catalytic effect Effects 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 239000000446 fuel Substances 0.000 description 3
- 229910002804 graphite Inorganic materials 0.000 description 3
- 239000010439 graphite Substances 0.000 description 3
- 229910052736 halogen Inorganic materials 0.000 description 3
- 150000002367 halogens Chemical class 0.000 description 3
- 238000010438 heat treatment Methods 0.000 description 3
- 239000002127 nanobelt Substances 0.000 description 3
- 229910000484 niobium oxide Inorganic materials 0.000 description 3
- URLJKFSTXLNXLG-UHFFFAOYSA-N niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Nb+5].[Nb+5] URLJKFSTXLNXLG-UHFFFAOYSA-N 0.000 description 3
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 3
- 229910052721 tungsten Inorganic materials 0.000 description 3
- 239000010937 tungsten Substances 0.000 description 3
- WXNZTHHGJRFXKQ-UHFFFAOYSA-N 4-chlorophenol Chemical class OC1=CC=C(Cl)C=C1 WXNZTHHGJRFXKQ-UHFFFAOYSA-N 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- 238000006555 catalytic reaction Methods 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 239000002105 nanoparticle Substances 0.000 description 2
- 239000002135 nanosheet Substances 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 230000004044 response Effects 0.000 description 2
- 238000010189 synthetic method Methods 0.000 description 2
- 238000012876 topography Methods 0.000 description 2
- ISPYQTSUDJAMAB-UHFFFAOYSA-N 2-chlorophenol Chemical compound OC1=CC=CC=C1Cl ISPYQTSUDJAMAB-UHFFFAOYSA-N 0.000 description 1
- 229910002900 Bi2MoO6 Inorganic materials 0.000 description 1
- 229910021276 Co2V2O7 Inorganic materials 0.000 description 1
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 1
- 229910003378 NaNbO3 Inorganic materials 0.000 description 1
- 238000001237 Raman spectrum Methods 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 229910001308 Zinc ferrite Inorganic materials 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 150000001336 alkenes Chemical class 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000010953 base metal Substances 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 239000012876 carrier material Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 230000001112 coagulating effect Effects 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 239000011258 core-shell material Substances 0.000 description 1
- 230000008878 coupling Effects 0.000 description 1
- 238000010168 coupling process Methods 0.000 description 1
- 238000005859 coupling reaction Methods 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 210000002249 digestive system Anatomy 0.000 description 1
- 230000005518 electrochemistry Effects 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 235000019441 ethanol Nutrition 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 229910001385 heavy metal Inorganic materials 0.000 description 1
- 238000007210 heterogeneous catalysis Methods 0.000 description 1
- 238000003837 high-temperature calcination Methods 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- NNGHIEIYUJKFQS-UHFFFAOYSA-L hydroxy(oxo)iron;zinc Chemical compound [Zn].O[Fe]=O.O[Fe]=O NNGHIEIYUJKFQS-UHFFFAOYSA-L 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 229910052744 lithium Inorganic materials 0.000 description 1
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 1
- 229910052753 mercury Inorganic materials 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000002114 nanocomposite Substances 0.000 description 1
- 210000005036 nerve Anatomy 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- 239000005416 organic matter Substances 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 238000006303 photolysis reaction Methods 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 230000007096 poisonous effect Effects 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 230000002035 prolonged effect Effects 0.000 description 1
- 102000004169 proteins and genes Human genes 0.000 description 1
- 108090000623 proteins and genes Proteins 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 230000029058 respiratory gaseous exchange Effects 0.000 description 1
- MUPJWXCPTRQOKY-UHFFFAOYSA-N sodium;niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Na+].[Nb+5] MUPJWXCPTRQOKY-UHFFFAOYSA-N 0.000 description 1
- 230000006641 stabilisation Effects 0.000 description 1
- 238000011105 stabilization Methods 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- PBCFLUZVCVVTBY-UHFFFAOYSA-N tantalum pentoxide Inorganic materials O=[Ta](=O)O[Ta](=O)=O PBCFLUZVCVVTBY-UHFFFAOYSA-N 0.000 description 1
- 239000004408 titanium dioxide Substances 0.000 description 1
- 230000001988 toxicity Effects 0.000 description 1
- 231100000419 toxicity Toxicity 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/20—Vanadium, niobium or tantalum
-
- B01J35/39—
-
- B01J35/399—
-
- B01J35/50—
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/34—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation
- B01J37/341—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation
- B01J37/344—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation of electromagnetic wave energy
- B01J37/346—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation of electromagnetic wave energy of microwave energy
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/70—Treatment of water, waste water, or sewage by reduction
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/20—Heavy metals or heavy metal compounds
- C02F2101/22—Chromium or chromium compounds, e.g. chromates
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
- C02F2101/345—Phenols
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/30—Wastewater or sewage treatment systems using renewable energies
- Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy
Abstract
The present invention relates to a kind of Nb (OH)5Nano wire/redox graphene composite photo-catalyst and the preparation method and application thereof.The active component of the catalyst is Nb (OH)5With redox graphene, structure is Nb (OH)5Nano wire is evenly distributed on stratiform redox graphene.The present invention is with Nb2O5For niobium source, GO is carrier and template, the In-situ reaction object of niobates nano wire and redox graphene is made through microwave process for synthesizing, acid is exchanged is replaced into hydrogen ion by the metal ion between niobate layers, niobic acid nano wire and redox graphene compound are obtained, is calcined up to Nb (OH)5Nano wire/redox graphene composite photo-catalyst.The preparation method of the present invention is simply time saving, and material morphology is uniform, and synthesis condition is easily-controllable, is suitble to industrialized mass production.It utilizes Nb (OH)5Highly toxic hexavalent chrome reduction while removing Phenol for Waste Water pollutant under room temperature radiation of visible light, can be trivalent chromium, achieve the purpose that high purification combined pollution waste water by nano wire/redox graphene composite photo-catalyst.
Description
Technical field
The invention belongs to photocatalyst technology fields, and in particular to a kind of Nb (OH)5Nano wire/redox graphene is multiple
Closing light catalyst and the preparation method and application thereof.
Background technology
Pattern has greatly in heterogeneous catalysis, solar energy conversion with fields such as optical electro-chemistry with controllable composite material is formed
Potential using value (H.Liu, et al.3D Bi2MoO6 Nanosheet/TiO2 Nanobelt Heterostructure:
Enhanced Photocatalytic Activities and Photoelectrochemical Performance,ACS
Catal.2015,5,4530-4536；X.S.Zhao,et al.Nitrogen-Doped Titanate-Anatase Core-
Shell Nanobelts with Exposed{101}Anatase Facets and Enhanced Visible Light
Photocatalytic Activity,J.Am.Chem.Soc.2012,134,5754-5757；Korea Spro at etc., nano heterojunction light
Catalysis material produces solar energy fuel progress, Chinese Journal of Inorganic Chemistry .2015, and 30,1121-1130；Lee's generation is superfine, three-dimensional point
The controlledly synthesis of level structure titanium dioxide nano material is in progress with application study, and chemical industry is in progress .2015, and 34,4272-4279).
Wherein, one-dimensional nano structure such as nano wire, nanometer rods and nanobelt etc., because with compared with big L/D ratio and specific surface area, contributing to
Photogenerated charge can effectively inhibit compound (F.Q.Huang, the et of photo-generate electron-hole pair in the fast transferring of catalyst surface
al.Gray Ta2O5 Nanowires with Greatly Enhanced Photocatalytic Performance,ACS
Appl.Mater.Interfaces 2016,8,122-127；Zhou Guowei etc., 1-dimention nano TiO2Morphological control and photocatalysis
Application study is in progress, New Chemical Materials .2013, and 41,177-180).It can also increase catalyst by building one-dimensional nano structure
Surface defect, for catalysis reaction more active sites are provided, to improve its photocatalysis performance.
Graphene or redox graphene (RGO) are special in conjunction with its because having good electric conductivity and chemical stability
Monoatomic layer planar structure and its high-specific surface area, be widely used in light frequently as the carrier material of nano particle and urge
Fields (J.S.Wu, et al.Graphene and the Graphene-like Molecules such as change, energy storage and fuel cell:
Prospects in Solar Cells,J.Am.Chem.Soc.2016,138,1095-1102；Z.Y.Fan,et
al.Comparing Graphene-TiO2 Nanowire and Graphene-TiO2 Nanoparticle Composite
Photocatalysts,ACS Appl.Mater.Interfaces 2012,4,3944-3950).Graphite oxide (GO) is system
The important presoma of standby graphene and RGO, because there is a large amount of oxygen-containing group (- OH ,-COOH ,-O-, C=O) on its surface so that GO
Strong coupling easily is generated with many oxides, to obtain graphene or RGO based composites.But only minority is ground at present
Study carefully the nanostructure for reporting and GO being used to prepare specific morphology as template, and the GO templates in these reports are follow-up
Heat treatment stages (Z.J.Fan, et al.Photocatalyst Interface are removed by high-temperature calcination
Engineering:Spatially Confined Growth of ZnFe2O4 within Graphene Networks as
Excellent Visible-Light-Driven Photocatalysts,Adv.Funct.Mater. 2015,25,7080-
7087；L.Q.Mai,et al.Graphene Oxide Templated Growth and Superior Lithium
Storage Performance of Novel Hierarchical Co2V2O7 Nanosheets,ACS Appl.
Mater.Interfaces 2016,8,2812-2818).Containing niobium material as photochemical catalyst, because of its environmental-friendly, high stabilization
Property and catalytic performance, by the extensive concern of researchers.It is relatively more to the research of base metal niobate photochemical catalyst at present,
And it is relatively fewer to the photocatalysis of crystal form or unformed niobium oxide research, and have synthesis niobium oxide base light in document report and urge
The method of agent uses expensive ethyl alcohol niobium (H.F.Shi, et al.Polymeric g-C more3N4 Coupled with
NaNbO3 Nanowires toward Enhanced Photocatalytic Reduction of CO2 into
Renewable Fuel,ACS Catal.2014,4,3637-3643；M.Qamar,et al.Single-Pot Synthesis
of<001>-Faceted N-Doped Nb2O5/Reduced Graphene Oxide Nanocomposite for
Efficient Photoelectrochemical Water Splitting,ACS Appl.Mater.Interfaces
2015,7,17954-17962), or pass through prolonged high-temperature heat treatment (J.H.Ye, et al.Nitrogen-Doped
Lamellar Niobic Acid with Visible Light-Responsive Photocatalytic Activity,
Adv. Mater.2008,20,3816-3819), the method for these synthesis niobium oxide is comparatively comparatively laborious, experiment condition not
It is easy to control.In recent years, microwave process for synthesizing is as a kind of new nano materials technology, have be quick on the draw, heated system it is equal
It even, the advantages that heating speed is fast, prepared sample topography is controllable, attracts widespread attention.The present invention using GO as carrier
With template, Nb (OH) is prepared using microwave process for synthesizing simple and easy to control5Nano wire/there is not been reported for RGO composite photo-catalysts.
Phenolic compound in waste water is a kind of plasm poisonous substance, can make protein coagulating, to nerve system of human body and life
State environment has prodigious potential hazard, while the presence of the heavy metal ion such as chromium, mercury, lead is often accompanied by phenols wastewater,
Wherein water-soluble Cr (VI) has very strong toxicity, and oxidisability is very strong, can be to productions such as the skin of people, breathing and digestive systems
It is raw to seriously endanger.Water body combined pollution caused by phenols organic pollution and Cr (VI) are common not only makes its behavior in the environment
It converts increasingly complex, is removed while further increasing the difficulty of governance of polluted-water, therefore study Organic-inorganic composite pollutant
It is of great significance to the comprehensive treatment of waste water.
Invention content
The object of the present invention is to provide a kind of Nb (OH) with visible light catalysis activity5Nano wire/reduction-oxidation graphite
Alkene composite photo-catalyst and the preparation method and application thereof, the Nb (OH)5Nano wire/redox graphene composite photo-catalyst exists
Phenol for Waste Water pollutant and reduction of hexavalent chromium can be removed under radiation of visible light simultaneously.
In summary：In order to achieve the above object, technical scheme is as follows：
A kind of Nb (OH)5Nano wire/redox graphene composite photo-catalyst is with constituent mass percentages：
Redox graphene mass content is 0.5~10.0%, remaining group is divided into Nb (OH)5；Its active component is Nb
(OH)5With redox graphene, microstructure is Nb (OH)5Nano wire is evenly distributed on stratiform redox graphene.
A kind of Nb (OH)5The preparation method of nano wire/redox graphene composite photo-catalyst, includes the following steps：
The first step, by Nb2O5It is dispersed in aqueous slkali, stirs 0.5~2h at room temperature, graphite oxide is then added thereto
Aqueous solution, at room temperature 0.5~2h of ultrasound mixing suspension is made；
Mixing suspension made from the first step is transferred in polytetrafluoroethylene (PTFE) microwave reaction tank by second step, seals postposition
0.5~2h is reacted in microwave reactor；
After third step, microwave reaction, the suspension in retort is filtered by vacuum, gained solid content is used respectively
150mL dilute hydrochloric acid washs 3 times, is then repeatedly washed with deionized water again, until filtrate pH is about 7, obtained solid part is 60
~90 DEG C of dryings, and the powder sample after drying is calcined into 1~2h for 300~400 DEG C in tube furnace, Nb (OH) is made5Nanometer
Line/redox graphene composite photo-catalyst.
By adjusting Nb2O5Addition, the concentration of graphene oxide water solution, alkaline concentration, microwave power with react
The preparation conditions such as time can control Nb (OH)5The pattern and composition of nano wire/redox graphene composite photo-catalyst.
Further, the Nb in the first step2O5Can be Nb2O5Powder or Nb2O5Colloid.
Further, aqueous slkali used is NaOH or KOH solution in the first step, the molar concentration of aqueous slkali is 8~
16 mol/L。
Further, graphene oxide used had both been Nb (OH) in the first step5The carrier of nano wire distribution, while again
It is Nb (OH)5The template of nanowire growth.
Further, the mass concentration of graphene oxide water solution used is 0.5~10mg/mL in the first step.
Further, the power of microwave reactor used is 200~500W in the second step.
Further, a concentration of 0.02~1mol/L of dilute hydrochloric acid used in the second step.
A kind of Nb (OH)5Nano wire/redox graphene composite photo-catalyst removes useless simultaneously under visible light illumination
Application in water in terms of phenolic comp ' ds pollution and reduction of hexavalent chromium.
Advantageous effect：
(1) graphene oxide being added in preparation process of the invention, is both Nb (OH)5The carrier of nano wire distribution, together
When be also Nb (OH)5The addition of the template of nanowire growth, graphene oxide can make Nb (OH)5Nano wire dispersibility with
One property significantly improves.
(2) preparation process of the invention is simply time saving, and Nb (OH) is realized using microwave process for synthesizing5Predecessor niobates nanometer
The In-situ reaction of line and redox graphene is conducive to that Nb (OH) is made5The composite photo-catalyst that nano wire is evenly distributed.
(3) Nb (OH) in made composite catalyst5Nano wire has larger draw ratio, and passes through In-situ reaction Nb
(OH)5Close interfacial contact is formd between nano wire and redox graphene, may advantageously facilitate point of photo-generate electron-hole
From improving its photocatalytic activity.
(4) photocatalysis removal phenolic comp ' ds pollution in reduction Cr the reacting of (VI), Nb (OH)5The hydroxyl of nanowire surface
It can be reacted with phenol organic matter and generate surface complexes, be conducive to the absorption and removal of phenolic comp ' ds pollution.Meanwhile surface complexes
Charge migration occurs after absorbing visible light, the photoelectron of generation passes through Nb (OH)5Nano wire is transferred to redox graphene table
Face, Cr (VI) that can effectively in reducing waste water.
(5) Nb (OH) of the invention5Nano wire/redox graphene composite photo-catalyst goes down for radiation of visible light
When except phenolic comp ' ds pollution with reduction Cr (VI), good catalytic effect is shown.Nb prepared by the present invention (OH)5Nano wire/RGO
Composite catalyst is used for light degradation phenolic comp ' ds pollution and the reaction condition of reduction Cr (VI) is：Phenols containing a concentration of 20mg/L
Cr (VI) the solution 50mL of pollutant and a concentration of 40mg/L are as analog composite pollutant effluents, Nb (OH)5Nano wire/RGO is multiple
Conjunction catalyst amount is 50mg, and lower 1~3h of radiation of visible light is stirred at room temperature, and the degradation rate of phenolic comp ' ds pollution is higher than 90%, simultaneously
The reduction rate of Cr (VI) is also up to 90% or more, wherein visible light source used can be furnished with 420nm cut-off type optical filters
300W xenon lamps, 300W halogen tungsten lamps or sunlight.The present invention method under radiation of visible light, normal temperature and pressure and condition of neutral pH i.e.
It can implement, and the photochemical catalyst is also with good stability, be catalyzed above-mentioned combined pollution waste water solution, continuous cycle 6 times, phenol
The degradation rate of pollutant remains to reach 85% and 82% with the reduction rate of Cr (VI), in waste water in terms of combined pollutant removal
With important potential application.
(6) Nb (OH) of the invention5Nano wire/redox graphene composite photo-catalyst, cannot be only used for the same time
Degrading phenol pollutant and reduction Cr (VI), and also have very greatly in fields such as solar cell, photodissociation aquatic products hydrogen, catalytic carriers
Application potential.
Description of the drawings
Fig. 1 is Nb (OH) in embodiment 15The x-ray diffraction pattern of nano wire/redox graphene composite photo-catalyst
Figure, shows the nanometer threadiness Nb (OH) in prepared catalyst5For undefined structure；
Fig. 2 is Nb (OH) in embodiment 25The raman spectrum of nano wire/redox graphene composite photo-catalyst, shows
Contain RGO in composite catalyst；
Fig. 3 is Nb (OH) in embodiment 15The transmission electron microscope picture of nano wire/redox graphene composite photo-catalyst,
Show Nb (OH)5Nano wire is evenly distributed in sheet redox graphene surface；
Fig. 4 is Nb (OH) in embodiment 35The recycling effect of nano wire/redox graphene composite photo-catalyst
Figure.
Specific implementation mode
Below in conjunction with specific embodiment, the invention will be further described:
Embodiment 1：
A kind of Nb (OH)5The preparation method of nano wire/redox graphene composite photo-catalyst：
Based on mass fraction, redox graphene mass content is 1.0%, Nb (OH)5For armorphous nano line, length
3 μm, diameter 100nm.The preparation method of the composite photo-catalyst is as follows：
By 1g Nb2O5Powder is placed in the KOH solution of the 10mol/L of 70mL, and 10mL is added thereto after 1h is stirred at room temperature
1.0 mg/mL graphene oxide water solution, at room temperature ultrasound 0.5h obtain mixing suspension；Gained mixing suspension is turned
It moves in polytetrafluoroethylene (PTFE) microwave reaction tank, sealing is placed in microwave reactor reacts 1.5h under 300W power；After cooling,
Suspension in retort is filtered by vacuum, gained solid content washs 3 with the dilute hydrochloric acid of the 0.02mol/L of 150mL respectively
It is secondary, it is then repeatedly washed with deionized water again, until filtrate pH is about 7, after the 80 DEG C of dryings of obtained solid object, places it in tubular type
350 DEG C of calcining 1.5h, are made Nb (OH) in stove5Nano wire/redox graphene composite photo-catalyst.
Application examples 1
Composite photocatalyst for degrading phenolic comp ' ds pollution is tested with reduction Cr (VI)：It is added in one glass reactor and contains 20mg/L
Phenol and 40mg/L Cr (VI) solution 50mL, above-mentioned made Nb (OH)5Nano wire/RGO composite catalyst 50mg, to be furnished with
As light source lower radiation of visible light 2h is stirred at room temperature, the degradation rate of phenol is 94%, Cr in the 300W xenon lamps of 420nm optical filters
(VI) reduction rate is 92%.
Comparative example 1
Blank Nb (OH)5The preparation of nano wire：Detailed process is same as Example 1, is only added without graphene oxide water
Solution, obtained catalyst are still unformed Nb (OH)5, but when its scanning electron microscopic picture is displayed without graphene oxide, it is made
Sample topography is inhomogenous, existing Nb (OH)5Nano wire, while also larger block-like Nb (OH)5.And aerobic fossil in embodiment 1
In the presence of black alkene, Nb (OH) in the composite photo-catalyst of preparation5To be uniformly dispersed, the nano wire that pattern is uniform.This shows this hair
The graphene oxide being added in bright preparation process is in addition to as Nb (OH)5Carrier outside, also to Nb (OH)5The growth of nano wire rises
To the effect of template.
Blank Nb (OH)5Degrading phenol pollutant is tested with reduction Cr (VI)：It is added in one glass reactor and contains 20mg/L
Phenol and 40mg/L Cr (VI) solution 50mL, above-mentioned made blank Nb (OH)5Catalyst 50mg, using in embodiment 1
After identical light source irradiates the same time, the reduction rate that the degradation rate of phenol is 33%, Cr (VI) is 25%, this experimental result
Significantly lower than Nb (OH) in embodiment 15The photocatalysis result of nano wire/redox graphene.
Embodiment 2：
A kind of Nb (OH)5The preparation method of nano wire/redox graphene composite photo-catalyst：
Based on mass fraction, redox graphene mass content is 2.5%, Nb (OH)5For armorphous nano line, length
3.5 μm, diameter 80nm.The preparation method of the composite photo-catalyst is as follows：
By 2g Nb2O5Colloid is placed in the NaOH solution of 70mL 16mol/L, is added thereto after 0.5h is stirred at room temperature
The graphene oxide water solution of 5.0 mg/mL of 10mL, at room temperature ultrasound 2h obtain mixing suspension；By gained mixing suspension
It is transferred in polytetrafluoroethylene (PTFE) microwave reaction tank, sealing is placed in microwave reactor reacts 1h under 500W power；After cooling,
Suspension in retort is filtered by vacuum, gained solid content is washed 3 times with the dilute hydrochloric acid of the 1mol/L of 150mL respectively,
Then it is repeatedly washed with deionized water again, until filtrate pH is about 7, after the 70 DEG C of dryings of obtained solid object, places it in tube furnace
In 300 DEG C calcining 2h, be made Nb (OH)5Nano wire/redox graphene composite material.
Application examples 2
Composite photocatalyst for degrading phenolic comp ' ds pollution is tested with reduction Cr (VI)：It is added in one glass reactor and contains 20mg/L
4- chlorophenols and 40mg/L Cr (VI) solution 50mL, above-mentioned made Nb (OH)5Nano wire/RGO composite catalyst 50mg,
Using the 300W xenon lamps equipped with 420nm optical filters as light source, lower radiation of visible light 1.5h, the degradation rate of 4- chlorophenols is stirred at room temperature
Reduction rate for 96%, Cr (VI) is 95%.
Embodiment 3：
A kind of Nb (OH)5The preparation method of nano wire/redox graphene composite photo-catalyst：
Based on mass fraction, redox graphene mass content is 5.0%, Nb (OH)5For armorphous nano line, length
1.5 μm, diameter 120nm.The preparation method of the composite photo-catalyst is as follows：
By 0.5g Nb2O5Powder is placed in the KOH solution of 70mL 8mol/L, is added thereto after 1.5h is stirred at room temperature
The GO aqueous solutions of 2.5 mg/mL of 10mL, at room temperature ultrasound 1.5h obtain mixing suspension；Gained mixing suspension is transferred to
In polytetrafluoroethylene (PTFE) microwave reaction tank, sealing is placed in microwave reactor reacts 2h under 200W power；After cooling, to reaction
Suspension in tank is filtered by vacuum, and gained solid content washs 3 times with the dilute hydrochloric acid of the 0.1mol/L of 150mL respectively, then
It is repeatedly washed with deionized water, until filtrate pH is about 7, after the 60 DEG C of dryings of obtained solid object, is placed it in 400 in tube furnace again
DEG C calcining 1h, be made Nb (OH)5Nano wire/RGO composite photo-catalysts.
Application examples 3
Composite photocatalyst for degrading phenolic comp ' ds pollution is tested with reduction Cr (VI)：It is added in one glass reactor and contains 20mg/L
2,4- chlorophenesic acids (DCP) and 40mg/L Cr (VI) solution 50mL, above-mentioned made Nb (OH)5Nano wire/RGO is compound to be urged
Lower radiation of visible light 2h, the degradation of 2,4- chlorophenesic acids (DCP) is stirred at room temperature using 300W halogen tungsten lamps as light source in agent 50mg
The reduction rate that rate is 98%, Cr (VI) is 99%.
The Nb (OH) in system5Nano wire/redox graphene composite catalyst is separated by centrifugal filtration
Carry out second of circular response.The composite photo-catalyst isolated is put into clean glass reactor, rejoins 20mg/
2, the 4- chlorophenesic acids of L and Cr (VI) solution 50mL of 40mg/L are then turned on stirring and are irradiated with light source and react 2h, and 2,4- bis-
The reduction rate that the degradation rate of chlorophenol (DCP) is 95%, Cr (VI) is 97%.
Such circular response repeats five times, and reaction result is shown in Fig. 4.
Embodiment 4：
A kind of Nb (OH)5The preparation method of nano wire/redox graphene composite photo-catalyst：
Based on mass fraction, redox graphene mass content is 10.0%, Nb (OH)5It is long for armorphous nano line
4 μm of degree, diameter 70nm.The preparation method of the composite photo-catalyst is as follows：
By 1g Nb2O5Colloid is placed in the NaOH solution of 70mL 12mol/L, and 10mL is added thereto after 1h is stirred at room temperature
The graphene oxide water solution of 10.0 mg/mL, at room temperature ultrasound 2h obtain mixing suspension；Gained mixing suspension is shifted
Into polytetrafluoroethylene (PTFE) microwave reaction tank, sealing is placed in microwave reactor reacts 1.5h under 500W power；It is right after cooling
Suspension in retort is filtered by vacuum, and gained solid content washs 3 times with the dilute hydrochloric acid of 150mL0.5mol/L respectively, so
It is repeatedly washed with deionized water, until filtrate pH is about 7, after the 90 DEG C of dryings of obtained solid object, is placed it in tube furnace again afterwards
350 DEG C of calcining 1.5h, are made Nb (OH)5Nano wire/redox graphene composite photo-catalyst.
Application examples 4
Composite photocatalyst for degrading phenolic comp ' ds pollution is tested with reduction Cr (VI)：It is added in one glass reactor and contains 20mg/L
2,4- chlorophenesic acids and 40mg/L Cr (VI) solution 50mL, above-mentioned made Nb (OH)5Nano wire/RGO composite catalysts 50
Using 300W halogen tungsten lamps as light source lower radiation of visible light 2h is stirred at room temperature, the degradation rate of 2,4- chlorophenesic acids is 91%, Cr in mg
(VI) reduction rate is 92%.
Embodiment 5
A kind of Nb (OH)5The preparation method of nano wire/redox graphene composite photo-catalyst：
Based on mass fraction, redox graphene mass content is 0.5%, Nb (OH)5For armorphous nano line, length
4.5 μm, diameter 60nm.The preparation method of the composite photo-catalyst is as follows：
By 3g Nb2O5Powder is placed in the NaOH solution of 70mL 10mol/L, and 10mL is added thereto after 2h is stirred at room temperature
The graphene oxide water solution of 1.5 mg/mL, at room temperature ultrasound 1h obtain mixing suspension；Gained mixing suspension is transferred to
In polytetrafluoroethylene (PTFE) microwave reaction tank, sealing is placed in microwave reactor reacts 2h under 400W power；After cooling, to reaction
Suspension in tank is filtered by vacuum, and gained solid content washs 3 times with the dilute hydrochloric acid of 150mL 0.3mol/L respectively, then again
It is repeatedly washed with deionized water, until filtrate pH is about 7, after the 75 DEG C of dryings of obtained solid object, places it in tube furnace 300 DEG C
2h is calcined, Nb (OH) is made5Nano wire/redox graphene composite photo-catalyst.
Application examples 5
Composite photocatalyst for degrading phenolic comp ' ds pollution is tested with reduction Cr (VI)：It is added in one glass reactor and contains 20mg/L
2,4,6- trichlorophenol, 2,4,6,-Ts and 40mg/L Cr (VI) solution 50mL, above-mentioned made Nb (OH)5Nano wire/RGO composite catalysts
Lower radiation of visible light 2h is stirred at room temperature using the xenon lamp equipped with 420nm optical filters as light source in 50mg, 2,4,6- trichlorophenol, 2,4,6,-Ts
The reduction rate that degradation rate is 93%, Cr (VI) is 92%.
Embodiment 6
A kind of Nb (OH)5The preparation method of nano wire/redox graphene composite photo-catalyst：
Based on mass fraction, redox graphene mass content is 5.0%, Nb (OH)5For armorphous nano line, length
4 μm, diameter 75nm.The preparation method of the composite photo-catalyst is as follows：
By 1g Nb2O5Colloid is placed in the KOH solution of 70mL 12mol/L, and 10mL is added thereto after 1.5h is stirred at room temperature
The graphene oxide water solution of 5.0 mg/mL, at room temperature ultrasound 1.5h obtain mixing suspension；Gained mixing suspension is shifted
Into polytetrafluoroethylene (PTFE) microwave reaction tank, sealing is placed in microwave reactor reacts 1.5h under 450W power；It is right after cooling
Suspension in retort is filtered by vacuum, and gained solid content is washed 3 times with the dilute hydrochloric acid of the 0.6mol/L of 150mL respectively,
Then it is repeatedly washed with deionized water again, until filtrate pH is about 7, after the 80 DEG C of dryings of obtained solid object, places it in tube furnace
In 400 DEG C calcining 1h, be made Nb (OH)5Nano wire/redox graphene composite photo-catalyst.
Application examples 6
Composite photocatalyst for degrading phenolic comp ' ds pollution is tested with reduction Cr (VI)：It is added in one glass reactor and contains 20mg/L
2,4,6- trichlorophenol, 2,4,6,-Ts and 40mg/L Cr (VI) solution 50mL, above-mentioned made Nb (OH)5Nano wire/RGO composite catalysts
Lower radiation of visible light 1h is stirred at room temperature using the xenon lamp equipped with 420nm optical filters as light source in 50mg, 2,4,6- trichlorophenol, 2,4,6,-Ts
The reduction rate that degradation rate is 100%, Cr (VI) is 98%.
Embodiment 7
Nb (OH) is prepared using the synthetic method in embodiment 65Nano wire/redox graphene composite photo-catalyst.
Application examples 7
Composite photocatalyst for degrading phenolic comp ' ds pollution is tested with reduction Cr (VI)：It is added in one glass reactor and contains 20mg/L
Phenol and 40mg/L Cr (VI) solution 50mL, the Nb (OH) prepared in embodiment 65Nano wire/RGO composite catalysts
Then reactor is put under sunlight by 50mg, select the 10 AM of illumination abundance to 4 periods of afternoon, stir lower shine
Reaction 3h is penetrated, the reduction rate that the degradation rate of phenol is 92%, Cr (VI) is 93%.
Embodiment 8
Nb (OH) is prepared using the synthetic method in embodiment 65Nano wire/redox graphene composite photo-catalyst.
Application examples 8
Composite photocatalyst for degrading phenolic comp ' ds pollution is tested with reduction Cr (VI)：It is added in one glass reactor and contains 20mg/L
2,4,6- trichlorophenol, 2,4,6,-Ts and 40mg/L Cr (VI) solution 50mL, the Nb (OH) prepared in embodiment 65Nano wire/RGO is multiple
Catalyst 50mg is closed, then reactor is put under sunlight, selects the 10 AM of illumination abundance to 4 periods of afternoon,
The lower irradiation reaction 2.5h of stirring, the reduction rate that the degradation rate of 2,4,6- trichlorophenol, 2,4,6,-Ts is 99%, Cr (VI) is 98%.
Although above the present invention is described in detail with a general description of the specific embodiments,
On the basis of the present invention, it can be made some modifications or improvements, this will be apparent to those skilled in the art.Cause
This, these modifications or improvements, belong to the scope of protection of present invention without departing from theon the basis of the spirit of the present invention.
Claims (8)
1. a kind of Nb (OH)5The preparation method of nano wire/redox graphene composite photo-catalyst, which is characterized in that its component
Mass percent is calculated as：
Redox graphene mass content is 0.5~10.0%, remaining group is divided into Nb (OH)5；Its active component is Nb (OH)5
With redox graphene, microstructure is Nb (OH)5Nano wire is evenly distributed on stratiform redox graphene；
The preparation method, includes the following steps：
The first step, by Nb2O5It is dispersed in aqueous slkali, stirs 0.5~2h at room temperature, graphene oxide water is then added thereto
Solution, at room temperature 0.5~2h of ultrasound mixing suspension is made；
Mixing suspension made from the first step is transferred in polytetrafluoroethylene (PTFE) microwave reaction tank by second step, and sealing is placed on micro-
0.5~2h is reacted in wave reactor；
After third step, microwave reaction, the suspension in retort is filtered by vacuum, gained solid content is respectively with 150
ML dilute hydrochloric acid washs 3 times, is then repeatedly washed with deionized water again, until filtrate pH is about 7, obtained solid part 60~
90 DEG C of dryings, and the powder sample after drying is calcined into 1~2h for 300~400 DEG C in tube furnace, Nb (OH) is made5Nanometer
Line/redox graphene composite photo-catalyst.
2. a kind of Nb (OH) according to claim 15The preparation side of nano wire/redox graphene composite photo-catalyst
Method, which is characterized in that the Nb in the first step2O5Can be Nb2O5Powder or Nb2O5Colloid.
3. a kind of Nb (OH) according to claim 15The preparation side of nano wire/redox graphene composite photo-catalyst
Method, which is characterized in that aqueous slkali used is NaOH or KOH solution in the first step, and the molar concentration of aqueous slkali is 8~16
mol/L。
4. a kind of Nb (OH) according to claim 15The preparation side of nano wire/redox graphene composite photo-catalyst
Method, which is characterized in that graphene oxide used had both been Nb (OH) in the first step5The carrier of nano wire distribution, while again
It is Nb (OH)5The template of nanowire growth.
5. a kind of Nb (OH) according to claim 15The preparation side of nano wire/redox graphene composite photo-catalyst
Method, which is characterized in that the mass concentration of graphene oxide water solution used is 0.5~10mg/mL in the first step.
6. a kind of Nb (OH) according to claim 15The preparation side of nano wire/redox graphene composite photo-catalyst
Method, which is characterized in that the power of microwave reactor used is 200~500W in the second step.
7. a kind of Nb (OH) according to claim 15The preparation side of nano wire/redox graphene composite photo-catalyst
Method, which is characterized in that a concentration of 0.02~1mol/L of dilute hydrochloric acid used in the third step.
8. a kind of Nb (OH) prepared by preparation method as described in claim 15Nano wire/redox graphene complex light is urged
Agent removes the application in terms of Phenol for Waste Water pollutant and reduction of hexavalent chromium simultaneously under visible light illumination.
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